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.

2017, Engelmann, Ronny, Ansmann, Albert, Horn, Stefan, Seifert, Patric, Althausen, Dietrich, Tesche, Matthias, Esselborn, Michael, Fruntke, Julia, Lieke, Kirsten, Freudenthaler, Volker, Gross, Silke

A 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.

2017, Heintzenberg, Jost, Hermann, Markus, Weigelt, Andreas, Kapustin, Vladimir, Anderson, Bruce, Thornhill, Kenneth, Van Velthoven, Peter, Zahn, Andreas, Brenninkmeijer, Carl

This 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.

2017, Freudenthaler, Volker, Esselborn, Michael, Wiegner, Matthias, Heese, Birgit, Tesche, Matthias, Ansmann, Albert, Müller, Detlef, Althausen, Dietrich, Wirth, Martin, Fix, Andreas, Ehret, Gerhard, Knippertz, Peter, Toledano, Carlos, Gasteiger, Josef, Garhammer, Markus, Seefeldner, Meinhard

Vertical profiles of the linear particle depolarization ratio of pure dust clouds were measured during the Saharan Mineral Dust Experiment (SAMUM) at Ouarzazate, Morocco (30.9◦N, –6.9◦E), close to source regions in May–June 2006, with four lidar systems at four wavelengths (355, 532, 710 and 1064 nm). The intercomparison of the lidar systems is accompanied by a discussion of the different calibration methods, including a new, advanced method, and a detailed error analysis. Over the whole SAMUM periode pure dust layers show a mean linear particle depolarization ratio at 532 nm of 0.31, in the range between 0.27 and 0.35, with a mean Ångström exponent (AE, 440–870 nm) of 0.18 (range 0.04–0.34) and still high mean linear particle depolarization ratio between 0.21 and 0.25 during periods with aerosol optical thickness less than 0.1, with a mean AE of 0.76 (range 0.65–1.00), which represents a negative correlation of the linear particle depolarization ratio with the AE. A slight decrease of the linear particle depolarization ratio with wavelength was found between 532 and 1064 nm from 0.31 ± 0.03 to 0.27 ± 0.04.

2017, Ng, Nga Lee, Brown, Steven S., Archibald, Alexander T., Atlas, Elliot, Cohen, Ronald C., Crowley, John N., Day, Douglas A., Donahue, Neil M., Fry, Juliane L., Fuchs, Hendrik, Griffin, Robert J., Guzman, Marcelo I., Herrmann, Hartmut, Hodzic, Alma, Iinuma, Yoshiteru, Jimenez, José L., Kiendler-Scharr, Astrid, Lee, Ben H., Luecken, Deborah J., Mao, Jingqiu, McLaren, Robert, Mutzel, Anke, Osthoff, Hans D., Ouyang, Bin, Picquet-Varrault, Benedicte, Platt, Ulrich, Pye, Havala O.T., Rudich, Yinon, Schwantes, Rebecca H., Shiraiwa, Manabu, Stutz, Jochen, Thornton, Joel A., Tilgner, Andreas, Williams, Brent J., Zaveri, Rahul A.

Oxidation of biogenic volatile organic compounds (BVOC) by the nitrate radical (NO3) represents one of the important interactions between anthropogenic emissions related to combustion and natural emissions from the biosphere. This interaction has been recognized for more than 3 decades, during which time a large body of research has emerged from laboratory, field, and modeling studies. NO3-BVOC reactions influence air quality, climate and visibility through regional and global budgets for reactive nitrogen (particularly organic nitrates), ozone, and organic aerosol. Despite its long history of research and the significance of this topic in atmospheric chemistry, a number of important uncertainties remain. These include an incomplete understanding of the rates, mechanisms, and organic aerosol yields for NO3-BVOC reactions, lack of constraints on the role of heterogeneous oxidative processes associated with the NO3 radical, the difficulty of characterizing the spatial distributions of BVOC and NO3 within the poorly mixed nocturnal atmosphere, and the challenge of constructing appropriate boundary layer schemes and non-photochemical mechanisms for use in state-of-the-art chemical transport and chemistry–climate models. This review is the result of a workshop of the same title held at the Georgia Institute of Technology in June 2015. The first half of the review summarizes the current literature on NO3-BVOC chemistry, with a particular focus on recent advances in instrumentation and models, and in organic nitrate and secondary organic aerosol (SOA) formation chemistry. Building on this current understanding, the second half of the review outlines impacts of NO3-BVOC chemistry on air quality and climate, and suggests critical research needs to better constrain this interaction to improve the predictive capabilities of atmospheric models.

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.

2017, Kahn, Ralph, Petzold, Andreas, Wendisch, Manfred, Bierwirth, Eike, Dinter, Tilman, Esselborn, Michael, Fiebig, Marcus, Heese, Birgit, Knippertz, Peter, Müller, Detlef, Schladitz, Alexander, Von Hoyningen-HUENE, Wolfgang

Coincident observations made over the Moroccan desert during the Sahara mineral dust experiment (SAMUM) 2006 field campaign are used both to validate aerosol amount and type retrieved from multi-angle imaging spectroradiometer (MISR) observations, and to place the suborbital aerosol measurements into the satellite’s larger regional context. On three moderately dusty days during which coincident observations were made, MISR mid-visible aerosol optical thickness (AOT) agrees with field measurements point-by-point to within 0.05–0.1. This is about as well as can be expected given spatial sampling differences; the space-based observations capture AOT trends and variability over an extended region. The field data also validate MISR’s ability to distinguish and to map aerosol air masses, from the combination of retrieved constraints on particle size, shape and single-scattering albedo. For the three study days, the satellite observations (1) highlight regional gradients in the mix of dust and background spherical particles, (2) identify a dust plume most likely part of a density flow and (3) show an aerosol air mass containing a higher proportion of small, spherical particles than the surroundings, that appears to be aerosol pollution transported from several thousand kilometres away.

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.

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.

2017, Hermann, M., Brenninkmeijer, C.A.M., Slemr, F., Heintzenberg, J., Martinsson, B.G., Schlager, H., Van Velthoven, P.F.J., Wiedensohler, A., Zahn, A., Ziereis, H.

Particle number and mass concentrations of submicrometer aerosol particles were determined for the upper troposphere over the mid-latitude North Atlantic within the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container project (CARIBIC, http://www.caribic-atmospheric.com). Between May 2001 and April 2002, 22 flights from Germany to the Caribbean were conducted using an automated measurement container on a B767 passenger aircraft. Spatial and seasonal probability distributions for ultrafine and Aitken mode particles as well as mass concentrations of particulate sulphur in 8–12 km altitude are presented. High particle number concentrations (mostly 2500–15 000 particles cm-3 STP) are particularly found in summer over the western North Atlantic Ocean close to the North American continent. The distributions together with an analysis of particle source processes show that deep vertical transport is the dominant process leading to most of the events with high particle number concentrations (8000 particles cm-3 STP) for ultrafine particles as well as for Aitken mode particles. This study emphasizes the importance of deep vertical transport and cloud processing for the concentration of aerosol particles in the upper troposphere.